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Mühr-Ebert, E.L.; Wagner, F.; Walther, C. |
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Title |
Speciation of uranium: Compilation of a thermodynamic database and its experimental evaluation using different analytical techniques |
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Journal Article |
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Year |
2019 |
Publication  |
Applied Geochemistry |
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100 |
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213-222 |
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Environmental hazards are caused by uranium mining legacies and enhanced radioactivity in utilized groundwater and surface water resources. Knowledge of uranium speciation in these waters is essential for predicting radionuclide migration and for installing effective water purification technology. The validity of the thermodynamic data for the environmental media affected by uranium mining legacies is of utmost importance. Therefore, a comprehensive and consistent database was established according to current knowledge. The uranium data included in the database is based on the NEA TDB (Guillaumont et al., 2003) and is modified or supplemented as necessary e.g. for calcium and magnesium uranyl carbonates. The specific ion interaction theory (Brönsted, 1922) is used to estimate activity constants, which is sufficient for the considered low ionic strengths. The success of this approach was evaluated by comparative experimental investigations and model calculations (PHREEQC (Parkhurst and Appelo, 1999)) for several model systems. The waters differ in pH (2.7–9.8), uranium concentration (10−9-10−4 mol/L) and ionic strength (0.002–0.2 mol/L). We used chemical extraction experiments, ESI-Orbitrap-MS and time-resolved laser-induced fluorescence spectroscopy (TRLFS) to measure the uranium speciation. The latter method is nonintrusive and therefore does not change the chemical composition of the investigated waters. This is very important, because any change of the system under study may also change the speciation. |
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0883-2927 |
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THL @ christoph.kuells @ muhr-ebert_speciation_2019 |
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142 |
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Ruiz, O.; Thomson, B.; Cerrato, J.M.; Rodriguez-Freire, L. |
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Title |
Groundwater restoration following in-situ recovery (ISR) mining of uranium |
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Journal Article |
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Year |
2019 |
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Applied Geochemistry |
Abbreviated Journal |
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109 |
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104418 |
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Aquifer stabilization, Ground water restoration, In-situ leach mining, In-situ recovery, Uranium |
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From 1950 through the early 1980’s New Mexico accounted for roughly half of domestic uranium (U) production for the nuclear power industry and the nation’s weapon programs. Increased interest in nuclear energy has led to proposals for renewed development using both underground mining and uranium in situ recovery (ISR). When feasible, ISR greatly reduces waste generated by the mining and milling processes, however, the ability to restore ground water to acceptable quality after ISR ends is uncertain. This research investigated two methods of stabilizing an aquifer following ISR. Batch and column studies were performed to evaluate chemical and biological methods of stabilization. Columns packed with ore were first leached with an aerated NaHCO3 ground water solution to simulate ISR. Constituents present at elevated concentrations after leaching included molybdenum (Mo), selenium (Se), U, and vanadium (V). Chemical stabilization was studied by passing a phosphate (PO43-) amended solution through the ore to achieve passivation of mineral surfaces by P precipitates. Microbial stabilization was studied by passing a lactate solution through the ore to stimulate growth of anaerobic metal- and sulfate-reducing organisms to reduce U and other elements to less soluble phases. Analyses of the solids from the columns after completion of these experiments by X-ray photo electron spectroscopy (XPS) identified phosphate on samples near the column inlet of the chemically stabilized columns. Microbial populations were characterized by Illumina DNA sequencing and confirmed the presence of metal- and sulfate-reducing organisms. Neither chemical nor microbial stabilization method achieved contaminant immobilization, which is believed due to limited mixing of the stabilization solutions with the contaminated leach solutions. These results emphasize that ground water hydrodynamics, especially mixing, must be considered in aquifer restoration of soluble constituents. |
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THL @ christoph.kuells @ ruiz_groundwater_2019 |
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153 |
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Botha, R.; Lindsay, R.; Newman, R.T.; Maleka, P.P.; Chimba, G. |
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Radon in groundwater baseline study prior to unconventional shale gas development and hydraulic fracturing in the Karoo Basin (South Africa) |
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Journal Article |
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2019 |
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Applied Radiation and Isotopes |
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147 |
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7-13 |
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The prospect of unconventional shale gas development in the semi-arid Karoo Basin (South Africa) has created the prerequisite to temporally characterise the natural radioactivity in associated groundwater which is solely depended on for drinking and agriculture purposes. Radon (222Rn) was the primary natural radionuclide of interest in this study; however, supplementary radium (226Ra and 228Ra) in-water measurements were also conducted. A total of 53 aquifers spanning three provinces were studied during three separate measurement campaigns from 2014 to 2016. The Karoo Basin’s natural radon-in-water levels can be characterised by a minimum of 1 ± 1 Bq/L (consistent with zero or below LLD), a maximum of 183 ± 18 Bq/L and mean of 41 ± 5 Bq/L. The mean radon-in-water levels for shallow aquifers were systematically higher (55 ± 10 Bq/L) compared to deep (14 ± 3 Bq/L) or mixed aquifers (20 ± 6 Bq/L). Radon-in-water activity concentration fluctuations were predominantly observed from shallow aquifers compared to the generally steady levels of deep aquifers. A collective seasonal mean radon-in-water levels increase from the winter of 2014 (44 ± 8 Bq/L) to winter of 2016 (61 ± 16 Bq/L) was noticed which could be related to the extreme national drought experienced in 2015. Radium-in-water (228Ra and 226Ra) levels ranged from below detection level to a maximum of 0.008 Bq/L (226Ra) and 0.015 Bq/L (228Ra). The 228Ra/226Ra ratio was characterised by a minimum of 0.93, a maximum of 6.5 and a mean value of 3.3 ± 1.3. Developing and improving baseline naturally occurring radionuclide groundwater databases is vital to study potential radiological environmental impacts attributed to industrial processes such as hydraulic fracturing or mining. |
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0969-8043 |
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THL @ christoph.kuells @ botha_radon_2019 |
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169 |
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Karaimeh, S.A. |
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Maintaining desert cultivation: Roman, Byzantine, and Early Islamic water-strategies at Udhruh region, Jordan |
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Journal Article |
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2019 |
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Journal of Arid Environments |
Abbreviated Journal |
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166 |
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108-115 |
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Irrigation, Qanat, Cultivation, Arid environment, Nabataean, Jordan |
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The site of Udhruh is located in the arid desert of southern Jordan, about 15 km to the east of Petra. The site was built by the Nabataeans but expanded by the Romans (as a defensive site) and was continuously occupied until the Early Islamic period. It receives less than the 200 mm of annual precipitation, which is crucial for agricultural cultivation. Archaeological evidence from earlier excavations together with new data from several survey projects indicate that areas around Udhruh were cultivated throughout the Roman, Byzantine, and Early Islamic periods (300 BCE–800 CE). The fundamental question is: how did the people of Udhruh sustain their community in the desert, and how did they transform the desert into arable land? The landscape could be utilised thanks to sophisticated water management and irrigation techniques. At least four underground qanat systems were identified providing Udhruh with access to groundwater. At the terminal end of the qanat systems, several types of closed surface channels conveyed the water to reservoirs, which subsequently distributed the water to the field systems. The water systems of Udhruh differ from the well-known Nabataean systems in the surrounding area. As Udhruh was taken over by the Roman army in 106 CE, this study analyses how the Nabataean water systems continued to function and adapt through the Roman and Byzantine periods. A complete understanding of Udhruh’s water systems helps to reconstruct past land use, agricultural activity, and irrigation practices in a currently arid region. |
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0140-1963 |
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THL @ christoph.kuells @ Alkaraimeh2019108 |
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271 |
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Boulesteix, T.; Cathelineau, M.; Deloule, E.; Brouand, M.; Toubon, H.; Lach, P.; Fiet, N. |
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Ilmenites and their alteration products, sinkholes for uranium and radium in roll-front deposits after the example of South Tortkuduk (Kazakhstan) |
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Journal Article |
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2019 |
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Journal of Geochemical Exploration |
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206 |
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106343 |
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The approximate determination of average Ra/U disequilibria in orebodies is one of the most common causes of errors in U reserve estimations. In roll-front deposits, the disequilibria are however frequently distributed following complex geometries, which must be fully understood to prevent major U reserve overestimates and costly unproductive extractive operations. The processes responsible for disruption of the radioactive equilibria and the U and Ra carriers in such complex natural systems remain poorly constrained. In this contribution, we propose an innovative approach, mixing orebody to sub-grain scale studies to unravel the distribution of U and Ra and the processes responsible for their concentration and uncoupling. Using mineral separations, gamma spectrometry and mineral-chemical analyses, we identified the Fe-Ti clusters (altered ilmenite + pyrite/marcasite) as the microsites for coffinite precipitation and Ra concentration. To understand the influence of such clusters on the distribution of U and Ra at the deposit scale, whole-rock Ra/U disequilibria were measured and mapped at a series of ten drill holes along a profile crosscutting the studied roll-front. The main Ra/U disequilibria are encountered around the mineralization in low U content zones. They are controlled by two main processes. (1) In the oxidized zones, the immobility of 230Th with respect to the U produces patches of Ra disequilibria (carried by the altered U minerals). (2) In the immediate vicinity of the roll-front, the dissolution of the mineralization produces an Ra flux trapped by the alteration products of ilmenites, as definitely confirmed by direct SIMS measurements. Such a process is responsible for the Ra disequilibria envelope located downstream of the richest ores, also known as Ra halo. The highest Ra/U ratios correspond to oxidized upstream samples, but most other high Ra/U ratios are from reduced downstream samples close to the mineralization. Such a low to medium U content envelope with high Ra/U ratios constitutes the main cause of U reserve overestimations. |
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0375-6742 |
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THL @ christoph.kuells @ boulesteix_ilmenites_2019 |
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181 |
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